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The goal of this research was to investigate the difference in behavior of hydrophilic and hydrophobic colloids during transport in two-phase flow, in general, and their attachment and remobilization characters, in particular. Experiments were performed in a hydrophobic polydimethylsiloxane (PDMS) micromodel. Water and fluorinert-FC43 were used as the two immiscible liquids. Given the fact that PDMS is a hydrophobic material, fluorinert was the wetting phase and water was the nonwetting phase in this micromodel. As model colloids, we used hydrophilic polystyrene carboxylate-modified microspheres (dispersible in water) and hydrophobic fluorous-modified silica microspheres (dispersible in fluorinert) in separate experiments. Using a confocal laser scanning microscope, we directly observed fluid distribution and colloid movement within pores of the micromodel. We also obtained concentration breakthrough curves by measuring the fluorescent intensities in the outlet of the micromodel. The breakthrough curves during steady-state flow showed that the colloid attachment rate is inversely related to the background saturation of the fluid in which the colloids were dispersed. Our visualization results showed that the enhanced attachment of hydrophilic colloids at lower water saturations was due to the retention at the fluorinert-water interface and fluorinert-water-solid contact lines. This effect was observed to be much less in the case of hydrophobic colloids (dispersed in fluorinert). In order to explain the colloids behavior, we calculated interaction potential energies of colloids with PDMS surfaces, fluid-fluid interfaces, and fluid-fluid-solid contact lines. Also, balance of forces that control colloid, including DLVO, hydrodynamic, and surface tension forces, were determined. Our calculations showed that there is a stronger repulsive energy barrier between hydrophobic colloids and fluorinert-water interface and solid-fluid interface, compared with the hydrophilic colloids. Moreover, hydrophobic colloids were seen to aggregate due to strong attractive forces among them. These aggregates had even less tendency to attach to various interfaces, due to an increase in the corresponding energy barrier. For the colloid retention at fluid-fluid-solid contact lines, we found that the role of DLVO interactions was less important than capillary forces. During transient events, we found that attached colloids become remobilized. The colloids deposited on the solid-fluid interface were detached by the moving fluid-fluid-solid contact lines. But, this happened only when the liquid containing colloids was being displaced by the other liquid. We simulated breakthrough curves using a model based on a coupled system of equations for two-phase flow, advection-dispersion of colloids, adsorption to and desorption from fluid-fluid interfaces and fluid-solid interfaces. Very good agreements were obtained among measured breakthrough curves, visualization results, and numerical modeling.

Removal of model viruses by dune recharge was studied at a field site in the dune area of Castricum, Netherlands. Recharge water was dosed with bacteriophages MS2 and PRD1 for 11 days at a constant concentration in a 10- by 15-m compartment that was isolated in a recharge basin. Breakthrough was monitored for 120 days at six wells with their screens along a flow line. Concentrations of both phages were reduced about 3 log10 within the first 2.4 m and another 5 log10 in a linear fashion within the following 27 m. A model accounting for one-site kinetic attachment as well as first-order inactivation was employed to simulate the bacteriophage breakthrough curves. The major removal process was found to be attachment of the bacteriophages. Detachment was very slow. After passage of the pulse of dosed bacteriophages, there was a long tail whose slope corresponds to the inactivation rate coefficient of 0.07–0.09 day−1 for attached bacteriophages. The end of the rising and the start of the declining limbs of the breakthrough curves could not be simulated completely, probably because of an as yet unknown process.

[1] We investigated transport of viruses through saturated and unsaturated sand columns. Unsaturated experiments were conducted under conditions of uniform saturation and steady state water flow. The water saturation ranged from 1 to 0.5. Bacteriophages MS2 and ϕX174 were used as surrogates for pathogenic viruses in these studies. Phosphate-buffered solutions with different pH values (7.5, 6.2, 5.5, and 5) were utilized. Virus transport was modeled assuming first-order kinetic adsorption for interactions to the solid-water interface (SWI) and the air-water interface (AWI). Under saturated conditions, virus retention increased as pH decreased, and a one-site kinetic model produced a good fit to the breakthrough curves. Under unsaturated conditions a two-site kinetic model was needed to fit the breakthrough curves satisfactorily. The second site was attributed to the adsorption of phages to the AWI. According to our results, ϕX174 exhibits a high affinity to the AWI at pH values below 6.6 (the isoelectric point of ϕX174). Although it is believed that MS2 is more hydrophobic than ϕX174, MS2 had a lower affinity to the AWI than ϕX174, presumably because of the lower isoelectric point of MS2, which is equal to 3.9. Under unsaturated conditions, viruses captured within the column could be recovered in the column outflow by resaturating and immediately draining the column. Draining columns under saturated conditions, however, did not result in any recovery of viruses. Therefore the recovery can be attributed to the release of viruses adsorbed to the AWI. Our results suggest that electrostatic interactions of viruses with the AWI are much more important than hydrophobicity.